Pure rotational spectrum of the NCCS radical studied by Fourier-transform microwave spectroscopy

Abstract

Pure rotational transitions of the NCCS radical, showing resolved fine and hyperfine splittings, have been observed by Fourier-transform microwave spectroscopy in a discharged supersonic jet of acetonitrile and carbon disulfide. Since the transitions have been observed at frequencies corresponding to the even multiples of the rotational constant, it is concluded that the NCCS radical has a bent structure in the ground electronic state, X̃ 2A′, and the Ka=0 ladder of the radical has been observed under the jet-cooled condition. Precise molecular constants, including the hyperfine constants of the nitrogen nucleus, are determined by a least-squares fit for the observed transition frequencies using a standard asymmetric top Hamiltonian. The determined rotational constant is compared with results of high-level ab initio calculations in order to confirm the spectral carrier to be the bent NCCS radical.